The photolysis of aqueous CS2 has been studied using subpicosecond transient absorption spectroscopy. CS2 was photolyzed at 6.2 eV and the fast formation and decay of the photoproducts were monitored from 6.2 to 3.96 eV. Upon excitation, aqueous CS2 dissociates into CS+S. However, 93%+/-2% of the fragments geminately recombine on the electronic ground state potential of CS2 within a few picosecond leaving only 7%+/-2% of the CS+S fragments separated 100 ps after the excitation. In the gas phase, most of the dissociation occurs on a triplet-state potential surface, and the high recombination yield observed in aqueous solution therefore indicates a strong, solvent-assisted coupling between this state and the singlet ground state of CS2. The vibrationally excited CS2 molecule formed by the recombination transfers its high excess energy to the surrounding water molecules in two processes with time constants 8.4+/-1 and 33+/-7 ps. The rotational reorientation time of ground state CS2 is 6+/-1 ps, suggesting a surprisingly strong interaction between the neutral, nonpolar CS2 and the surrounding water molecules.